CN114735796A - Iron-based nano flocculant and preparation method and application thereof - Google Patents
Iron-based nano flocculant and preparation method and application thereof Download PDFInfo
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- CN114735796A CN114735796A CN202210530796.6A CN202210530796A CN114735796A CN 114735796 A CN114735796 A CN 114735796A CN 202210530796 A CN202210530796 A CN 202210530796A CN 114735796 A CN114735796 A CN 114735796A
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 153
- 229910052742 iron Inorganic materials 0.000 title claims abstract description 52
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims abstract description 57
- 235000003891 ferrous sulphate Nutrition 0.000 claims abstract description 35
- 239000011790 ferrous sulphate Substances 0.000 claims abstract description 35
- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims abstract description 35
- 239000002351 wastewater Substances 0.000 claims abstract description 16
- 238000004065 wastewater treatment Methods 0.000 claims abstract description 5
- 238000003756 stirring Methods 0.000 claims description 89
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 30
- 238000001816 cooling Methods 0.000 claims description 19
- 239000007788 liquid Substances 0.000 claims description 13
- 238000000034 method Methods 0.000 claims description 13
- 238000000926 separation method Methods 0.000 claims description 13
- 239000000203 mixture Substances 0.000 claims description 9
- 239000006185 dispersion Substances 0.000 claims description 8
- 238000002156 mixing Methods 0.000 claims description 4
- 230000000694 effects Effects 0.000 abstract description 8
- 239000000243 solution Substances 0.000 description 62
- 239000000463 material Substances 0.000 description 18
- 230000000052 comparative effect Effects 0.000 description 10
- 239000002244 precipitate Substances 0.000 description 10
- 229920006395 saturated elastomer Polymers 0.000 description 8
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 238000009360 aquaculture Methods 0.000 description 2
- 244000144974 aquaculture Species 0.000 description 2
- 238000005034 decoration Methods 0.000 description 2
- 238000005189 flocculation Methods 0.000 description 2
- 230000016615 flocculation Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000010802 sludge Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229910017108 Fe—Fe Inorganic materials 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000000084 colloidal system Substances 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 230000003311 flocculating effect Effects 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 229920002401 polyacrylamide Polymers 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 239000002344 surface layer Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/52—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
- C02F1/5236—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities using inorganic agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/08—Nanoparticles or nanotubes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Landscapes
- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Organic Chemistry (AREA)
- Separation Of Suspended Particles By Flocculating Agents (AREA)
Abstract
The invention provides an iron-based nano flocculant, a preparation method and application thereof, belongs to the technical field of wastewater treatment, and is prepared by wrapping nano zero-valent iron with ferrous sulfate. The iron-based nano flocculant provided by the invention improves the treatment effect on the wastewater, and does not need to adjust the pH value of the wastewater.
Description
Technical Field
The invention belongs to the technical field of wastewater treatment, and particularly relates to an iron-based nano flocculant, and a preparation method and application thereof.
Background
Ferrous sulfate is a common flocculant which forms precipitates by electrically neutralizing, adsorbing and flocculating organic pollutants in an aqueous solution after hydrolysis to aggregate small-particle colloidal pollutants into large-particle colloids. In order to improve the flocculation effect of ferrous sulfate, the pH value of the wastewater needs to be adjusted to about 9.0 in advance. However, alkaline conditions rapidly accelerate Fe2+And rapidly generate Fe (OH)3Precipitation, whereby the effective fraction of colloidal precipitates acting on the wastewater is small and sludge is formedLarge output, high sludge treatment cost and the like.
Disclosure of Invention
In view of this, the invention aims to provide an iron-based nano-flocculant, a preparation method and an application thereof, and the iron-based nano-flocculant provided by the invention improves the treatment effect on wastewater.
In order to achieve the above purpose, the invention provides the following technical scheme:
the invention provides an iron-based nano flocculant, which is prepared by wrapping ferrous sulfate with nano zero-valent iron.
The invention also provides a preparation method of the iron-based nano flocculant in the technical scheme, which comprises the following steps:
1) dissolving ferrous sulfate in water to obtain a saturated ferrous sulfate solution; the temperature of the water is 50-70 ℃;
2) dispersing the nano zero-valent iron to obtain a dispersion solution, and mixing the dispersion solution with the saturated ferrous sulfate solution obtained in the step 1) under stirring to obtain a mixture;
3) and (3) cooling the mixture obtained in the step 3) to 5-15 ℃ while stirring, continuing stirring for 5-10 min, and performing solid-liquid separation to obtain the iron-based nano flocculant.
Preferably, the temperature of the water in the step 1) is 60 ℃.
Preferably, the volume ratio of the mass of the nanometer zero-valent iron in the step 2) to the saturated ferrous sulfate solution is 20-50 g: 1L.
Preferably, the volume ratio of the mass of the nano zero-valent iron to the saturated ferrous sulfate solution is 30-40 g: 1L.
Preferably, the stirring time of the step 2) is not more than 15 min.
Preferably, the stirring speed of the step 2) and the step 3) is 150-300 rpm.
The invention also provides the application of the iron-based nano flocculant in the technical scheme in wastewater treatment.
Preferably, the dosage of the iron-based nano flocculant in each liter of wastewater is 1-2 g.
Preferably, the iron-based nano-flocculant removes COD and SS in wastewater.
The invention provides an iron-based nano flocculant, which is prepared by wrapping ferrous sulfate with nano zero-valent iron. In the invention, the iron-based nano flocculant is used, ferrous sulfate is rapidly dissolved and forms Fe-Fe with nano zero-valent iron2+Cell system and oxidation of Fe to Fe3+The quantity of electrons provided being Fe2+3 times of the total amount of the raw materials, thereby greatly increasing the supply speed and the quantity of electrons and increasing the chemical flocculation effect. Meanwhile, the pH value of the sewage does not need to be adjusted in advance when the flocculant is used, and the nano zero-valent iron effectively slows down Fe3+The generation speed is increased, and the utilization rate of the material in the use process is improved.
Detailed Description
The invention provides an iron-based nano flocculant, which is prepared by wrapping ferrous sulfate with nano zero-valent iron.
In the invention, the water content of the iron-based nano flocculant is preferably 50% by mass.
The invention also provides a preparation method of the iron-based nano flocculant in the technical scheme, which comprises the following steps:
1) dissolving ferrous sulfate in water to obtain a saturated ferrous sulfate solution; the temperature of the water is 50-70 ℃;
2) dispersing the nano zero-valent iron to obtain a dispersion solution, and mixing the dispersion solution with the saturated ferrous sulfate solution obtained in the step 1) under stirring to obtain a mixture;
3) and (3) cooling the mixture obtained in the step 3) to 5-15 ℃ while stirring, continuing stirring for 5-10 min, and performing solid-liquid separation to obtain the iron-based nano flocculant.
Dissolving ferrous sulfate in water to obtain a saturated ferrous sulfate solution; the temperature of the water is 50-70 ℃.
In the present invention, the temperature of the water is preferably 60 ℃.
The method comprises the steps of dispersing nano zero-valent iron to obtain a dispersion solution, and mixing the dispersion solution and a saturated ferrous sulfate solution under stirring to obtain a mixture. In the invention, the stirring time is not more than 15min, which can cause the oxidation of the nano zero-valent iron. In the present invention, the stirring speed is preferably 150 to 300 rpm. In the present invention, the amount of the nano zero-valent iron is calculated as a dry amount of iron.
The dispersant used for dispersing the nano zero-valent iron is not particularly limited, and the ordinary reagent for dispersing the nano zero-valent iron, such as polyacrylamide, carboxymethyl cellulose and the like, can be used by the technical personnel in the field
In the invention, the volume ratio of the mass of the nanometer zero-valent iron to the saturated ferrous sulfate solution is preferably 20-50 g:1L, and more preferably 30-40 g: 1L.
The obtained mixture is cooled to 5-15 ℃ under stirring, then is continuously stirred for 5-10 min, and the iron-based nano flocculant is obtained after solid-liquid separation. In the invention, along with the reduction of the temperature of the solution, the solubility of the ferrous sulfate in the solution is also rapidly reduced, and supersaturated ferrous sulfate is gradually precipitated on the surface of the nano zero-valent iron. The solid-liquid separation method is not particularly limited, and the method can be carried out by a person skilled in the art according to conventional operation.
The invention also provides application of the iron-based nano flocculant in the technical scheme in wastewater treatment. In the invention, the dosage of the iron-based nano flocculant in each liter of wastewater is preferably 1-2 g. In the present invention, the iron-based nano-flocculant preferably removes COD and SS in wastewater. The COD represents the chemical oxygen demand and the SS represents the suspended matter.
The technical solutions provided by the present invention are described in detail below with reference to examples, but they should not be construed as limiting the scope of the present invention.
Example 1
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 60 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 20g/L, the stirring time is not more than 10min, and the stirring speed is 150 rpm;
(3) then, rapidly cooling the solution to 5 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 150 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min, and after stirring is finished, quickly performing solid-liquid separation on the solution to obtain a precipitate which is an iron-based nano flocculant and has the water content of 50%.
Example 2
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 60 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 30g/L, the stirring time is not more than 10min, and the stirring speed is 200 rpm;
(3) then, rapidly cooling the solution to 5 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 200 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 200rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Example 3
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 60 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 40g/L, the stirring time is not more than 10min, and the stirring speed is 250 rpm;
(3) then, rapidly cooling the solution to 5 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 250 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 250rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Example 4
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 60 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 50g/L, the stirring time is not more than 10min, and the stirring speed is 300 rpm;
(3) then, rapidly cooling the solution to 5 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 300 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 300rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Example 5
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 50 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 30g/L, the stirring time is not more than 10min, and the stirring speed is 200 rpm;
(3) then, rapidly cooling the solution to 10 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 200 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 200rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Example 6
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 70 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 30g/L, the stirring time is not more than 10min, and the stirring speed is 200 rpm;
(3) then, rapidly cooling the solution to 15 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 200 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 200rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Comparative example 1
Preparing an iron-based nano flocculant:
(1) firstly, preparing hot water at 40 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 30g/L, the stirring time is not more than 10min, and the stirring speed is 200 rpm;
(3) then, rapidly cooling the solution to 10 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 200 rpm;
(4) and when the temperature is reduced to the designated temperature, continuously stirring for 10min at the stirring speed of 200rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is the iron-based nano flocculant and has the water content of 50%.
Comparative example 2
Preparing an iron-based nano flocculant:
(1) preparing hot water at 90 ℃, then adding ferrous sulfate, and continuously stirring until the ferrous sulfate in the solution is saturated;
(2) dispersing nano zero-valent iron, adding the dispersed nano zero-valent iron material into a saturated ferrous sulfate solution, uniformly stirring, wherein the adding amount of the nano zero-valent iron material is 30g/L, the stirring time is not more than 10min, and the stirring speed is 200 rpm;
(3) then, rapidly cooling the solution to 20 ℃, and continuously stirring the solution in the cooling process, wherein the stirring speed is 200 rpm;
(4) and when the temperature is reduced to the specified temperature, continuously stirring for 10min at the stirring speed of 200rpm, and quickly performing solid-liquid separation on the solution after the stirring is finished to obtain a precipitate which is an iron-based nano flocculant and has the water content of 50%.
Application example
Taking the aquaculture wastewater as a removal object, adding the iron-based nano-flocculant prepared in the examples 1-6 and the iron-based nano-flocculant prepared in the comparative examples 1-2 according to 1.5g/L respectively, wherein the water content of the iron-based nano-flocculant is 50%, the reaction time is 5min, ferrous sulfate is used as the comparative example 3, and the rest is prepared by a conventional method. The results are shown in Table 1.
TABLE 1 results of COD and SS removal from wastewater
| COD，mg/L | SS，mg/L | |
| Raw aquaculture wastewater composition | 7860 | 1267 |
| Example 1 | 781 | 55.9 |
| Example 2 | 472 | 35.7 |
| Example 3 | 389 | 24.1 |
| Example 4 | 233 | 12.5 |
| Example 5 | 505 | 49.7 |
| Example 6 | 498 | 48.9 |
| Comparative example 1 | 1024 | 117.9 |
| Comparative example 2 | 1147 | 142.8 |
| Comparative example 3 | 3629 | 755 |
As can be obtained from the table 1, (1) when other parameters are consistent, the more the amount of the added nano zero-valent iron is, the better the treatment effect on the wastewater is, but the preparation cost is comprehensively considered, and the adding amount of the nano zero-valent iron is 30-40 g: 1L; (2) the temperature difference of the solution determines the amount of ferrous sulfate precipitated on the surface of the material. In examples 5 and 6, the temperature is low when the ferrous sulfate solution is dissolved, and the temperature is high when the ferrous sulfate solution is cooled, so that the ferrous sulfate amount precipitated on the surface layer of the nano zero-valent iron is low, and the removal effect is influenced. The same problem is caused by the higher temperature reduction and control of the solution in the comparative example 7 and the comparative example 8. Also, when the hot water temperature is too high, oxidation of ferrous sulfate during stirring may be accelerated, resulting in poor effects. (3) Compared with the comparative example 3, the composite material can greatly improve the treatment effect on the wastewater.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (10)
1. An iron-based nano flocculant is characterized in that ferrous sulfate is wrapped by nano zero-valent iron to obtain the iron-based nano flocculant.
2. The preparation method of the iron-based nano flocculant according to claim 1, which is characterized by comprising the following steps:
1) dissolving ferrous sulfate in water to obtain a saturated ferrous sulfate solution; the temperature of the water is 50-70 ℃;
2) dispersing the nano zero-valent iron to obtain a dispersion solution, and mixing the dispersion solution with the saturated ferrous sulfate solution obtained in the step 1) under stirring to obtain a mixture;
3) and (3) cooling the mixture obtained in the step 3) to 5-15 ℃ while stirring, continuing stirring for 5-10 min, and performing solid-liquid separation to obtain the iron-based nano flocculant.
3. The method of claim 2, wherein the water of step 1) has a temperature of 60 ℃.
4. The preparation method of claim 2, wherein the volume ratio of the mass of the nanoscale zero-valent iron in the step 2) to the saturated ferrous sulfate solution is 20-50 g: 1L.
5. The preparation method of claim 4, wherein the volume ratio of the mass of the nanoscale zero-valent iron to the saturated ferrous sulfate solution is 30-40 g: 1L.
6. The method according to claim 2, wherein the stirring time in step 2) is not more than 15 min.
7. The preparation method of claim 2, wherein the stirring speed of the step 2) and the step 3) is 150-300 rpm.
8. Use of the iron-based nanoflocculant of claim 1 in wastewater treatment.
9. The application of the iron-based nano flocculant as claimed in claim 8, wherein the dosage of the iron-based nano flocculant in each liter of wastewater is 1-2 g.
10. The use according to claim 8, wherein the iron-based nanoflocculant removes COD and SS from wastewater.
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| CN109449431A (en) * | 2018-12-16 | 2019-03-08 | 成都其其小数科技有限公司 | A method of preparing lithium battery size tunable cobalt phosphate lithium composite positive pole |
| KR102022936B1 (en) * | 2018-12-28 | 2019-09-20 | 에이치플러스에코 주식회사 | Preparation method of nano zero-valent Iron modified with PVP-VA |
| CN112844350A (en) * | 2021-01-06 | 2021-05-28 | 湖南工业大学 | Titanium-containing blast furnace slag loaded nano zero-valent iron material and preparation method and application thereof |
| CN114229870A (en) * | 2021-12-08 | 2022-03-25 | 宜宾锂宝新材料有限公司 | In-situ carbon-coated Prussian blue positive electrode material and preparation method and application thereof |
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